Computational studies on carbon nanostructures encapsulating metal atom clusters are[unreadable] proposed. This work is intended to aid the design of novel pharmaceutical nanodevices, namely[unreadable] Magnetic Resonance Imaging (MRI) and X-ray Imaging contrast agents as well as[unreadable] radiopharmaceuticals used for diagnostic or therapeutic purposes. These systems consist of[unreadable] closed shell carbon clusters enclosing metal atom or metal cluster cores as exemplified by[unreadable] recently detected metallofullerenes of composition MxSc3-xN@CN (x = 0-2) and (M1)X(M2)3-[unreadable] XN@CN (x = 1-3) where M, MI, M2 are lanthanide atoms and N = 68, 80. As suggested by[unreadable] experimental assessment, these complexes may provide safer and more efficient[unreadable] Pharmaceuticals for MRI, X-ray and radiographic applications than the commonly utilized metal -[unreadable] chelate compounds. Small clusters of magnetic metal atoms have been shown to exhibit[unreadable] significantly higher magnetic effects than single atoms. This makes carbon nanostructures[unreadable] encaging these clusters interesting candidates for MRI contrast agents. Similarly, a cluster of[unreadable] heavy lanthanide atoms confined by a fullerene shell will generate high X-ray contrast, as first[unreadable] test measurements have demonstrated. Further, radiopharmaceuticals based on fullerenes with[unreadable] radioactive metal cluster cores are envisaged as well as multifunctional species that contain[unreadable] core atoms with high magnetic moments, high atomic numbers and suitable radioactive decay[unreadable] properties. These current pioneering activities in the areas of mass-spectrometric experiment as[unreadable] well as pharmaceutical design can greatly benefit from computational simulations that aim at an[unreadable] in-depth understanding of the respective nanosystems from first principles. Thus, it is planned to[unreadable] use a variety of Density Functional Theory (DFT) procedures to interpret the carbon[unreadable] nanostructures with endohedral metal clusters identified in the laboratory. The proposed[unreadable] research will include metallofullerenes as well as carbon nanotubes enclosing 3d transition[unreadable] metal atom substructures. The in-depth understanding of these species from first principles will[unreadable] make it possible to propose novel units that optimally satisfy the requirements of MRI, X-ray[unreadable] Imaging, radiographic treatment or a combination of these three areas of clinical application.